Transition metal dichalcogenide (TMD) nanosheets have attracted attention as novel inorganic materials. Aiming to enhance their availability, we targeted the large‐scale synthesis of TMD solid‐solution nanosheets by liquid‐phase exfoliation. To prepare the nanosheets, bulk polycrystalline Mo 1− x W x S 2 was sonicated in dimethyl sulfoxide. Transmission electron microscopy and atomic force microscopy showed that few‐layer nanosheets were formed. UV–VIS spectroscopy showed that the band structure could be continuously tuned. Compared with mechanical cleaving, our exfoliation method facilitates larger‐scale production of nanosheets and should be useful for a wide range of applications, such as thin films and composite materials.